Isolating Chemical Reaction Mechanism as a Variable with Reactive Coarse-Grained Molecular Dynamics: Step-Growth versus Chain-Growth Polymerization

We present a general approach to isolate chemical reaction mechanism as an independently controllable variable across chemically distinct systems. Modern approaches to reduce the computational expense of molecular dynamics simulations often group multiple atoms into a single "coarse-grained&quo...

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Bibliographic Details
Published in:arXiv.org 2022-10
Main Authors: Karnes, John J, Weisgraber, Todd H, Cook, Caitlyn C, Wang, Daniel N, Crowhurst, Jonathan C, Fox, Christina A, Harris, Bradley S, Oakdale, James S, Faller, Roland, Shusteff, Maxim
Format: Article
Language:English
Subjects:
Addition polymerization
Chains (polymeric)
Chemical reactions
Group dynamics
Mechanical tests
Molecular dynamics
Reaction mechanisms
Simulation
Online Access:Get full text
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Summary:We present a general approach to isolate chemical reaction mechanism as an independently controllable variable across chemically distinct systems. Modern approaches to reduce the computational expense of molecular dynamics simulations often group multiple atoms into a single "coarse-grained" interaction site, which leads to a loss of chemical resolution. In this work we convert this shortcoming into a feature and use identical coarse-grained models to represent molecules that share non-reactive characteristics but react by different mechanisms. As a proof of concept we use this approach to simulate and investigate distinct, yet similar, trifunctional isocyanurate resin formulations that polymerize by either chain- or step-growth. Since the underlying molecular mechanics of these models are identical, all emergent differences are a function of the reaction mechanism only. We find that the microscopic morphologies resemble related all-atom simulations and that simulated mechanical testing reasonably agrees with experiment.
ISSN:2331-8422
DOI:10.48550/arxiv.2210.01758